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Title: Crystal structure and magnetic properties of the Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, and Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14} langasites

We report the structural and magnetic characterizations of Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, and Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14}, compounds that are based on the mineral dugganite, which is isostructural to langasites. The magnetic part of the structure consists of layers of Co{sup 2+} triangles. Nuclear and magnetic structures were determined through a co-refinement of synchrotron and neutron powder diffraction data. In contrast to the undistorted P321 langasite structure of Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, a complex structural distortion yielding a large supercell is found for both Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14} and Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14}. Comparison of the three compounds studied along with the zinc analog Pb{sub 3}TeZn{sub 3}P{sub 2}O{sub 14}, also characterized here, suggests that the distortion is driven by Pb{sup 2+} lone pairs; as such, the Pb compounds crystallize in a pyroelectric space group, P2. Magnetic susceptibility, magnetization, and heat capacity measurements were performed to characterize the magnetic behavior. All three compounds become antiferromagnetic with Néel temperatures T{sub N}≈21 K (Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}), ≈13 K (Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}), and ≈8 K (Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14}), and they exhibit magnetic transitions at high applied magnetic fields,more » suggesting intrinsically complex magnetic behavior for tetrahedrally coordinated d{sup 7} Co{sup 2+} in this structure type. - Graphical abstract: Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14} and Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14} exhibit a triangles-of-triangles arrangement of the magnetic cations. Despite the Pb-induced crystallographic distortion, all of these materials exhibit competing antiferromagnetic and ferromagnetic interactions that lead to complex high field magnetism. - Highlights: • Nuclear and magnetic structures of Ba{sub 3}TeCo{sub 3}P{sub 2}O{sub 14}, Pb{sub 3}TeCo{sub 3}P{sub 2}O{sub 14} and Pb{sub 3}TeCo{sub 3}V{sub 2}O{sub 14}. • Structural characterization shows complex Pb-induced distortion. • Distortion puts Pb-compounds into space group that allows potential multiferroicity. • Magnetic characterization shows competing magnetic interactions. • Triangles of triangles motif results in complex high-field magnetic behavior.« less
Authors:
 [1] ;  [2] ;  [3] ;  [1]
  1. Department of Chemistry, Princeton University, Princeton, NJ 08544 (United States)
  2. Quantum Condensed Matter Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831-6393 (United States)
  3. Department of Physics, Technical University of Denmark, 2800 Kgs. Lyngby (Denmark)
Publication Date:
OSTI Identifier:
22309052
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Solid State Chemistry; Journal Volume: 203; Other Information: Copyright (c) 2013 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ANTIFERROMAGNETISM; CATIONS; COBALT IONS; COMPARATIVE EVALUATIONS; INTERACTIONS; LAYERS; LEAD COMPOUNDS; LEAD IONS; MAGNETIC FIELDS; MAGNETIC SUSCEPTIBILITY; MAGNETIZATION; SPACE GROUPS; TRIGONAL LATTICES; ZINC